<br>打破中心对称的同形相界：高灵敏度和强压力响应非线性光开关的途径,Journal of the American Chemical Society

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打破中心对称的同形相界：高灵敏度和强压力响应非线性光开关的途径
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-04-09 , DOI: 10.1021/jacs.4c02002
Munan Hao _{1,

2} , Xu Chen ₁ , Tianping Ying ₁ , Congcong Chai _{1,

2} , Jiali Lu _{1,

2} , Qi Li _{1,

2} , Zhaolong Liu _{1,

2} , Mingzhang Yang _{1,

3} , Junjie Wang _{1,

3} , Ruijin Sun ₄ , Donghan Jia ₅ , Xinyu Wang ₅ , Huiyang Gou ₅ , Jian-Gang Guo ₁ , Shifeng Jin _{1,

3} , Xiaolong Chen _{1,

6}

Affiliation

对高性能压电材料的追求一直与对同形相界 (MPB) 的追求同义，但在铁电领域之外，MPB 的全部潜力在很大程度上尚未得到开发。在这项研究中，我们通过在中心对称和非中心对称化合物之间创建连续的基于分子的固溶体，揭示了一类新的MPB，例如(叔丁基铵) _{1– x} (叔戊基铵) _x FeCl ₄ (0 ≤ x ≤ 1 ），其中MPB是由于分子阳离子无序而形成的。在 MPB 附近，我们发现了一种异常灵敏的中心对称相非线性光学材料，能够在低至 0.12–0.27 GPa 的压力下激活，并产生从 0 到 18.8 倍 KH ₂的可调谐二次谐波发生 (SHG) 信号PO ₄ （KDP）。同时，同步加速器衍射实验揭示了在低压下出现的第三个竞争相（ P 2 ₁ 2 ₁ 2 ₁ ），在MPB附近形成三相点，从而深入了解非线性光学（NLO）开关行为的机制。这些发现强调了通过战略性设计新型 MPB 来利用对称破缺固溶体系统中的特殊物理特性的机会。

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Centrosymmetry-Breaking Morphotropic Phase Boundary: A Pathway to Highly Sensitive and Strong Pressure-Responsive Nonlinear Optical Switches

The quest for high-performance piezoelectric materials has been synonymous with the pursuit of the morphotropic phase boundary (MPB), yet the full potential of MPBs remains largely untapped outside of the realm of ferroelectrics. In this study, we reveal a new class of MPB by creating continuous molecular-based solid solutions between centro- and noncentrosymmetric compounds, exemplified by (tert-butylammonium)_1–x(tert-amylammonium)_xFeCl₄ (0 ≤ x ≤ 1), where the MPB is formed due to disorder of molecular cations. Near the MPB, we discovered an exceptionally sensitive nonlinear optical material in the centrosymmetric phase, capable of activation at pressures as low as 0.12–0.27 GPa, and producing tunable second-harmonic generation (SHG) signals from zero to 18.8 times that of KH₂PO₄ (KDP). Meanwhile, synchrotron diffraction experiments have unveiled a third competing phase (P2₁2₁2₁) appearing at low pressure, forming a triple-phase point near the MPB, thereby providing insight into the mechanism underpinning the nonlinear optical (NLO) switch behavior. These findings highlight the opportunity to harness exceptional physical properties in symmetry-breaking solid solution systems by strategically designing novel MPBs.

更新日期：2024-04-09

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